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Non-trivial Topological Surface States Regulation of 1T-OsCoTe2 Enables Selective C―C Coupling for Highly Efficient Photochemical CO2 Reduction Toward C2+ hydrocarbons

arXiv

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arXiv 2024年

作者： Wang, Kangwang Wu, Mingjie Yu, Peifeng Garces, Hector F. Liang, Ying Li, Longfu Zeng, Lingyong Li, Kuan Zhang, Chao Yan, Kai Luo, Huixia School of Materials Science and Engineering State Key Laboratory of Optoelectronic Materials and Technologies Guangdong Provincial Key Laboratory of Magnetoelectric Physics and Devices Key Lab of Polymer Composite & Functional Materials Sun Yat-sen University Guangzhou510275 China State Key Laboratory of New Textile Materials and Advanced Processing Technologies Wuhan Textile University Wuhan430200 China School of Engineering Brown University 182 Hope Street Providence United States The Basic Course Department Guangzhou Maritime University Guangzhou510800 China School of Environmental Science and Engineering Sun Yat-sen University Guangzhou510275 China

Despite ongoing research, the rational design of non-trivial topological semimetal surface states for the selective photocatalytic CO2 conversion into valuable products remains full of challenges. Herein, we present the synthesis of lattice-matched 1T-OsCoTe2 for the photoreduction upgrading of CO2 to tri-carbon (C2) alkane (propane, C2H2) by the integration of experimental work and theory prediction/calculation. Experimental studies suggested a high electron-based selectivity of 71.2% for C3H8 and an internal quantum efficiency of 54.6% at 380 nm. In-situ X-ray photoelectron spectroscopy and X-ray absorption fine structure spectroscopy demonstrated that Co and Os atoms coordinated with Te atoms enable an efficient Os―Te―Co electron transfer to activate the generation of *CH3, *CHOCO and *CH2OCOCO. Density functional theory calculations further confirmed Os―Te―Co electron bridging on the improved CO2 conversion kinetics. To our knowledge, this is the first report suggesting the role of Os atoms in accelerating the photocatalytic CO2 conversion activity of the topological semimetal 1T-OsCoTe2 Copyright © 2024, The Authors. All rights reserved.

关键词： Surface states

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MOF负载Weel抑制剂实现p53突变胆囊癌的合成致死靶向治疗

引用

science Bulletin 2024年第9期69卷 1286-1301页

作者：郦仕杰 Sarun Juengpanich Win Topatana 谢天傲侯丽丹朱怡远陈佳东单煜凯韩依纳陆子毅陈天恩 Charlie Topatana 张斌曹佳胜胡家豪严加费陈迎鑫顾臻俞计成蔡秀军陈鸣宇 Department of General Surgery Sir Run-Run Shaw HospitalZhejiang UniversityHangzhou 310016China School of Medicine Zhejiang UniversityHangzhou 310058China National Engineering Research Center of Innovation and Application of Minimally Invasive Instruments Sir Run-Run Shaw HospitalZhejiang UniversityHangzhou 310016China School of Materials Science and Engineering Zhejiang UniversityHangzhou 310058China Department of Chemistry Zhejiang UniversityHangzhou 310016China Department of Pathology Sir Run-Run Shaw HospitalZhejiang UniversityHangzhou 310016China International College Zhejiang UniversityHangzhou 310058China Institute of Advanced Magnetic Materials and International Research Center for EM Metamaterials College of Materials&Environmental EngineeringHangzhou Dianzi UniversityHangzhou 310018China Zhejiang Provincial Key Laboratory for Advanced Drug Delivery Systems College of Pharmaceutical SciencesZhejiang UniversityHangzhou 310058China National Key Laboratory of Advanced Drug Delivery and Release Systems Zhejiang UniversityHangzhou 310058China Liangzhu Laboratory Zhejiang UniversityHangzhou 311121China Jinhua Institute of Zhejiang University Jinhua 321299China MOE Key Laboratory of Macromolecular Synthesis and Functionalization Department of Polymer Science and EngineeringZhejiang UniversityHangzhou 310027China

Adavosertib(ADA)is a WEE1 inhibitor that exhibits a synthetic lethal effect on p53-mutated gallbladder cancer(GBC).However,drug resistance due to DNA damage response compensation pathways and high toxicity limits further ***,estrone-targeted ADA-encapsulated metal–organic frameworks(ADA@MOF-EPL)for GBC synthetic lethal treatment by inducing conditional factors are *** high expression of estrogen receptors in GBC enables ADA@MOF-EPL to quickly enter and accumulate near the cell nucleus through estrone-mediated endocytosis and release ADA to inhibit WEE1 upon entering the acidic tumor *** irradiation induces ADA@MOF-EPL to generate reactive oxygen species(ROS),which leads to a further increase in DNA damage,resulting in a higher sensitivity of p53-mutated cancer cells to WEE1 inhibitor and promoting cell death via conditional synthetic *** conditional factor induced by ADA@MOF-EPL further enhances the antitumor efficacy while significantly reducing systemic ***,ADA@MOF-EPL demonstrates similar antitumor abilities in other p53-mutated solid tumors,revealing its potential as a broad-spectrum antitumor drug.

关键词： Synthetic lethality Nanomedicine Sonodynamic therapy Gallbladder cancer Metal-organic frameworks DNA damage response

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Effect of Residual Lignin and Drying Temperature on Lignin-Containing Microfibrillated Cellulose Films

SSRN

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SSRN 2023年

作者： Li, Huisi Kulachenko, Artem Mathew, Aji P. Lindström, Mikael E. Sevastyanova, Olena KTH-Royal Institute of Technology Department of Fiber and Polymer Technology Teknikringen 56-58 StockholmSE-100 44 Sweden KTH-Royal Institute of Technology Department of Engineering Mechanics StockholmSE-100 44 Sweden Stockholm University Division of Materials and Environmental Chemistry Svante Arrhenius väg 16 C StockholmSE-10691 Sweden KTH-Royal Institute of Technology Wallenberg Wood Science Center – WWSC Department of Fiber and Polymer Technology Teknikringen 56-58 StockholmSE-100 44 Sweden

Recent developments in the production of nanocellulose have placed an emphasis on raw fibers that contain residual lignin, instead of bleached chemical pulps. In this work, lignin-containing microfibrillated cellulose (LMFC) was prepared using a scalable and environmentally friendly method from low-cost unbleached pulps. Pure microfibrillated cellulose fibers (MFC) were also produced from fully bleached industrial kraft pulp as a reference. Due to the presence of the charged carboxylic groups from hemicellulose and residual lignin, LMFC gel suspension showed a higher colloidal stability than the reference MFC. Furthermore, LMFC films exhibited enhanced hydrophobicity, thermal stability and improved mechanical properties compared to MFC films. The tensile strength and Young’s modulus of LMFC films dried at higher temperature further reached to 283 MPa and 15 GPa, respectively, suggesting that further strength improvement can be achieved from the thermoplasticity of lignin by tuning the drying conditions. Microfibrillated fibers also exhibited better cracking resistance at folding state due to the longer fibers. These high-performance films fabricated from unbleached pulps via a green and sustainable method have great potential as scalable, strong and biodegradable materials. © 2023, The Authors. All rights reserved.

关键词： Bleaching

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Dependence of adhesive friction on surface roughness and elastic modulus

arXiv

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arXiv 2021年

作者： Maksuta, Daniel Dalvi, Siddhesh Gujrati, Abhijeet Pastewka, Lars Jacobs, Tevis D.B. Dhinojwala, Ali Department of Biology Integrated Bioscience Program The University of Akron AkronOH44325 United States School of Polymer Science and Polymer Engineering The University of Akron AkronOH44325 United States Department of Mechanical Engineering and Materials Science University of Pittsburgh PittsburghPA15261 United States Department of Microsystems Engineering University of Freiburg Freiburg79110 Germany

When adhesive elastomeric materials slide over hard rough surfaces at low velocities, there are two primary dissipative mechanisms that control how friction changes with sliding velocity: viscoelastic dissipation and adhesive dissipation. To distinguish the contribution of these dissipative mechanisms we have measured frictional shear stresses for crosslinked polydimethylsiloxane (PDMS) on three different rough surfaces of similar surface chemistry across nearly six decades of sliding velocity. The results show that the observed friction is dominated by adhesive dissipation, rather than viscoelastic dissipation. Prior models for elastomer friction assume that roughness only influences adhesive dissipation via the amount of contact area;by contrast, we find that the roughness-induced oscillations occurring across all length scales from macroscopic to atomic influence the molecular processes governing the adhesive dissipation. While it was previously known that roughness-induced oscillations affected the viscoelastic dissipation;this is the first demonstration that these oscillations also control the behavior of the adhesive component of friction. Finally, while theory predicts that rough friction should be independent of elastic modulus, we show that a strong dependence on modulus, with the frictional shear stress scaling as E’1/2. When analyzed in this way, data from four different moduli and three different roughnesses collapse onto a universal curve to describe the velocity-dependent friction of soft materials. Taken together, this investigation sheds new light on the adhesive component of friction, and how it depends on the roughness and stiffness of the materials. © 2021, CC BY-NC-SA.

关键词： Surface roughness

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Growth of Biobrxi1-X Solid-Solutions with Tunable Band-Gaps on Carbon Fiber Cloth as Flexible Membrane-Shaped Photocatalyst for Purifying Antibiotic Wastewater

SSRN

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SSRN 2022年

作者： Li, Xiaolong Cai, Jiafeng Li, Maoquan Zhang, Lisha Chen, Zhigang Department of Interventional and Vascular Surgery Shanghai Tenth People’s Hospital Tongji University School of Medicine Shanghai200072 China State Key Laboratory for Modification of Chemical Fibers and Polymer Materials College of Environmental Science and Engineering Donghua University Shanghai201620 China College of Materials Science and Engineering Donghua University Shanghai201620 China

Integrated membranes with filtration and photocatalysis functions have attracted much attention for purifying the flowing wastewater, but the design and preparation of high-efficiency and low-cost membranes is still of great urgency. Herein, we report efficient recyclable BiOBr x I 1-x fibrous filter membranous photocatalyst prepared through the in-situ growth of BiOBr x I 1-x solid-solutions with tunable band-gaps on carbon fiber cloth (CFC). The fabrication was performed via a facile dipping-solvothermal synthesis of BiOBr x I 1-x solid-solutions nanoplates (size: ~500 nm;thickness: ~50 nm) on CFC with different I/Br ratios in the precursor solution. With the increase of I/Br ratio from 0 to 4, CFC/BiOBr x I 1-x solid-solutions exhibit a re-shifted in the photoabsorption edge from 420 to 600 nm, leading to the tuning of the band-gap from 2.49 to 1.81 eV. Under visible light illumination for 120 min, CFC/BiOBr x I 1-x solid-solutions have the tuned photocatalytic activity, where CFC/BiOBr 0.8 I 0.2 shows the highest degradation efficiency toward various antibiotics (such as levofloxacin (LVFX, 94.1%), ciprofloxacin (CIP, 94.5%), and tetracycline (TC, 98.9%)) as well as dyes (such as acid orange 7 (AO7, 91.4%). Especially, when CFC/BiOBr 0.8 I 0.2 is used as a flexible membrane to a construct multi-grade unit for treating the flowing sewage, the degradation efficiency of LVFX goes up from 3.9% in the first grade to 96.2% in tenth grade. Therefore, the present CFC/BiOBr 0.8 I 0.2 not only possesses great potential as a flexible membrane-shaped photocatalyst for purifying the flowing sewage efficiently but also provides some insights for developing new types of purifying membranes and devices. © 2022, The Authors. All rights reserved.

关键词： Efficiency

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Theory for Salt Transport in Charged Reverse Osmosis Membranes: Novel Analytical Equations for Desalination Performance and Experimental Validation

SSRN

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SSRN 2023年

作者： Biesheuvel, P.M. Rutten, S. Ryzhkov, I. Porada, S. Elimelech, M. Wetsus European Centre of Excellence for Sustainable Water Technology Netherlands Membrane Science & Technology University of Twente Netherlands Institute of Computational Modeling SB RAS Akademgorodok 50 Krasnoyarsk660036 Russia Siberian Federal University Svobodny 79 Krasnoyarsk660041 Russia Department of Process Engineering and Technology of Polymer and Carbon Materials Wroclaw University of Science and Technology Wyb. St. Wyspianskiego ´ 27 Wroclaw50-370 Poland Department of Chemical and Environmental Engineering Yale University United States

Reverse osmosis is one of the most successful membrane technologies for desalination and contaminant removal from water. To characterize membrane performance, standard testing uses membrane coupons and an NaCl solution in a lab-scale setup under controlled conditions. Ideally, experiments are done for a range of applied pressures and salt concentrations, with water flux and salt rejection measured in each experiment. This full dataset can then be checked for internal consistency, and all these data must then be described by a comprehensive theoretical framework. Parameters derived from this procedure, such as water and salt permeability, can then be compared to those obtained in other studies. If this theory correctly describes data for water flux salt fluxes, it can be applied in larger scale models for RO modules. Herein, we present a novel equation for salt flux that we derive from the full solution-friction theory. This equation interpolates between an equation for neutral membranes on the one hand, and an equation for highly charged membranes on the other hand, and thus it is more generally applicable. We apply this new equation to several datasets of seawater RO membranes, and we propose an accurate method to compare the salt permeability of different membranes. © 2023, The Authors. All rights reserved.

关键词： Reverse osmosis

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General validity of the exponential law for the effect of concentration polarization in reverse osmosis in a stirred-cell geometry, including an activity correction for 1:1 salt solutions

arXiv

引用

arXiv 2023年

作者： Biesheuvel, P.M. Porada, S. Ryzhkov, I. Elimelech, M. Wetsus European Centre of Excellence for Sustainable Water Technology Netherlands Department of Process Engineering and Technology of Polymer and Carbon Materials Wroclaw University of Science and Technology Wyb. St. Wyspiańskiego 27 Wroclaw50-370 Poland Institute of Computational Modeling SB RAS Akademgorodok 50 Krasnoyarsk660036 Russia Siberian Federal University Svobodny 79 Krasnoyarsk660041 Russia Department of Chemical and Environmental Engineering Yale University United States

Reverse osmosis (RO) is a method to desalinate water, where water containing salts is pushed through a membrane while salt ions are rejected by the membrane. Very important in the theory of mass transport in RO is the concentration polarization (CP) layer, which develops on the upstream side of the membrane because of a combination of salt convection and diffusion. Because of the CP-effect, the salt concentration at the membrane surface is higher than in the channel, and this increases the osmotic pressure there, and thus transmembrane water flux is reduced (the osmotic pressure acts against water flux), while salt leakage through the membrane increases. So it is very important to understand and describe the CP-layer accurately. We analyze a one-dimensional geometry, which is of relevance for a typical lab-scale RO setup using small membrane coupons where the solution on the feed side of the membrane is stirred. For this geometry, the standard film layer approach is often used that assumes a stagnant film layer of a defined thickness, which however does not exist in reality. We set up a model without that assumption but including refreshment of solution because of the flow of water along the membrane due to stirring. We show that the ‘exponential law’ for the CP-layer that is predicted by the the film model, also applies for this more accurate model. We further improve the model by including the activity coefficient of salt ions, as described by the Bjerrum theory that is based on ion-ion Coulombic interactions. We evaluate the original linearized Bjerrum theory as well as an extended Bjerrum equation that is valid up to 1.5 M salt concentration. We show how including this activity correction leads to a reduction of the diffusional driving force at high concentration, and thus the salt concentration at the membrane further increases. However, the effect can be easily included by reducing the CP-layer mass transfer coefficient by a fixed percentage. Copyright © 2023,

关键词： Reverse osmosis

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Heat-Activated Peroxydisulfate and Peroxymonosulfate-Mediated Degradation of Benzotriazole: Effects of Chloride and Ph on Kinetics, Pathways and Product Toxicity

SSRN

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SSRN 2022年

作者： Saha, Pradip Zhou, Chenyu Moradi, Mahsa Blokland, Marco Rijnaarts, Huub H.M. Bruning, Harry Department of Environmental Technology Wageningen University and Research P.O. Box 17 Wageningen6700 AA Netherlands Department of Chemical Engineering and Polymer Science Shahjalal University of Science and Technology Sylhet3114 Bangladesh Department of Environmental Health Engineering School of Public Health Tehran University of Medical Sciences Tehran Iran Wageningen Food Safety Research Wageningen University & Research P.O. Box 230 Wageningen6708 WB Netherlands

The impact of chloride (Cl⁻) in heat-activated peroxydisulfate (PS) and peroxymonosulfate (PMS) processes for benzotriazole (BTA) degradation was investigated. The PMS-mediated BTA degradation rate showed an optimum at a Cl⁻ concentration of 1000 mg/L, while Cl⁻ inhibited PS-mediated BTA degradation. BTA degradation was mainly driven by hydroxyl and sulfate radicals in both PS and PMS systems without Cl⁻. However, reactive chlorine species (RCS) significantly boosted the PMS system for BTA degradation in presence of Cl⁻. LC-MS/MS analysis identified forty-two transformation products (TPs) . Based on the TPs, polymerization, hydroxylation, benzene ring-opening, and carboxylic acid formation were hypothesized to be the main degradation mechanisms in the absence of Cl⁻, whereas chlorination, triazole ring-opening, and nitration were the additional degradation steps in presence of Cl⁻. Moreover, more chlorinated TPs were found in PMS/Cl⁻ system than in PS/Cl⁻ combination, which was also reflected in AOX and end-product toxicity analyses. The PMS/Cl⁻ process produced other undesirable by-products such as chlorates, while these were not detected in the PS/Cl⁻ process. This shows that PS and PMS-based advanced oxidation processes can act notably different from the aspect of toxic by-product formation, and need to be critically evaluated before applying for organic pollutant degradation under saline conditions. © 2022, The Authors. All rights reserved.

关键词： Degradation

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Vanadium remediation from polluted wastewater using a novel non-conventional adsorbent

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Results in engineering 2025年

作者： Manar Banwan Hasan Suha Anwer Ibrahim Nisreen Mizher Rahmah Thekra Atta Ibrahim Alaa Hani Alminshid Mohammed Nsaif Abbas Environmental Engineering Department College of Engineering Mustansiriyah University Baghdad Iraq Materials Engineering Department College of Engineering Mustansiriyah University Baghdad Iraq Department of Biology College of Education for Pure Sciences University of Diyala Diyala Iraq Polymer Research Unit College of Science Mustansiriyah University Baghdad Iraq

This investigation studies the utilization of buckthorn leaves as a low-cost and environmentally friendly adsorbent to remove vanadium from simulated wastewater. Experiments were conducted using batches under various operating conditions. The obtained results indicated that the vanadium recovery efficiency reached 81% and was in direct proportion to the pH, agitation speed, and contact time, and inversely with other variables, while adsorption capacity reaching 0.1 mg/g. The optimum conditions for vanadium removal using this novel adsorbent are 150 min, 12 g, 8.0 mg/L, 350 rpm, and 6 for contact time, adsorbent dosage, initial vanadium concentration, agitation speed, and pH, respectively, and 25°C, while maintaining stable performance overall experiments. Morphological characterization of the material indicated that the buckthorn leaves contained multiple functional groups that contributed effectively to the capture of vanadium ions from the contaminated solution, according to Fourier transform infrared spectroscopy (FT-IR) analysis. Field Emission Scanning Electron Microscopy (FESEM) examination revealed that the adsorption medium underwent significant changes due to the accumulation of target metal particles, and that the surface area decreased from 13.3 to 1.275 m²/g as a result of adsorption, according to the results obtained from the Brunauer, Emmett and Teller (BET)test. The results showed that the adsorption was spontaneous in the temperature range studied, that it had a negative entropy of 438 J/mol.K, and that it was exothermic with an enthalpy of 142.7 kJ/mol, which means that the adsorption is chemisorption. Kinetically the closest model to describing the adsorption was the intra-particle diffusion model, while Langmuir was the best model for representative of the obtained data isothermally compared to the other models, according to the correlation coefficients, which were 0.9907, 0.992, respectively.

关键词： Adsorption batch unit buckthorn leaves removal vanadium wastewater treatment

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Polydopamine/Polypyrrole Modified Graphite Felt Enhances Biocompatibility for Electroactive Bacteria and Power Density of Microbial Fuel Cell

SSRN

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SSRN 2022年

作者： Kim, Minsoo Li, Shuwei Kong, Da Seul Song, Young Eun Park, Soo-Yong Kim, Hyoung-Il Jae, Jungho Chung, Ildoo Kim, Jung Rae School of Chemical Engineering Pusan National University Busan46241 Korea Republic of Advanced Biofuel and Bioproducts Process Development Unit Lawrence Berkeley National Laboratory EmeryvilleCA94608 United States School of Civil & Environmental Engineering Yonsei University Seoul03722 Korea Republic of Department of Polymer Science and Engineering Pusan National University Busan46241 Korea Republic of

The interactions between the microbes and the surface of an anode play an important role in capturing the respiratory electrons from bacteria in a microbial fuel cell (MFC). The chemical and electrochemical characteristics of the carbon material influences biofilm growth and direct electron transfer in MFCs. This study examined the electrodeposition of polydopamine (PDA), and polypyrrole (PPY) on graphite felt electrode (GF). The MFC with the modified PDA/PPY-GF reached 920 mW/m2, which was 1.5, 1.17, and 1.18 times higher than those of the GF, PDA-GF, and PPY-GF, respectively. PDA has superior hydrophilicity and adhesive force biofilm formation, while PPY provides electrochemically active sites for microbial electron transfer. Raman spectroscopy, Fourier transform infrared spectroscopy(FT-IR), Brunauer–Emmett–Teller surface area measurements(BET), and contact angle analysis revealed the enhanced physicochemical properties of the carbon electrode. These results show that co-doped PDA/PPY provides a strategy for electroactive biofilm development and improving bioelectrochemical performance in realistic MFC reactors. © 2022, The Authors. All rights reserved.

关键词： Electrodeposition

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